ACS Applied Materials & Interfaces
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2021
·
IF 9.229
Yuhan Sun,Minghui Li,Xiaolei Qu,Shourong Zheng,Pedro J. J. Alvarez,Heyun Fu
A stable catalyst, Pt/carbon nanotube (CNT) coated with N-doped carbon (Pt/CNT@CN), was designed to reduce selenite (Se(IV)) in water to elemental selenium by liquid-phase catalytic hydrogenation. Commercial Pt/C, pristine Pt/CNT, and carbon-coated Pt/CNT (Pt/CNT@C) were used for benchmarking. The Pt particles in Pt/CNT@CN were completely embedded beneath the coatings to minimize leaching and were not easily accessible to Se(IV). However, Schottky–Mott-type metal–carbon junctions that activate H2 were formed on the coated catalyst, facilitating effective reduction of Se(IV). The initial activity of Pt/CNT@CN (900.5 mg L–1 gcat–1 h–1) was two times higher than that of commercial Pt/C (448.6 mg L–1 gcat–1 h–1). The commercial Pt/C and uncoated Pt/CNT lost their initial activities during reuse and were almost inactive after 10 cycles due to significant Pt leaching (>90%) during the reaction and acid-washing regeneration processes. Pt/CNT@CN maintained 33% of the initial activity after the first cycle and stabilized over the following 9 cycles due to effective protection of Pt particles by carbon coatings. After 10 cycles, the activity of Pt/CNT@CN was over 20 times higher than that of Pt/C and uncoated Pt/CNT. Overall, catalytic hydrogenation using carbon-coated-supported Pt catalysts is an effective and promising approach to remove Se(IV) in water.
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INORGANIC CHEMISTRY
·
2018
·
IF 4.7
Syed S. Razi,Yun Hee Koo,Woojae Kim,Wenbo Yang,Zhijia Wang,Habtom Gobeze,Francis D’Souza,Jianzhang Zhao,Dongho Kim
A boron dipyrromethane (BDP)-containing Pt(II)–Schiff base complex (Pt-BDP), showing ping-pong singlet–triplet energy transfer, was synthesized, and the detailed photophysical properties were investigated using various steady-state and time-resolved transient spectroscopies. Femtosecond/nanosecond transient absorption spectroscopies demonstrated that, upon selective excitation of the BDP unit in Pt-BDP at 490 nm, Förster resonance energy transfer from the BDP unit to the Pt(II) coordination center occurred (6.7 ps), accompanied by an ultrafast intersystem crossing at the Pt(II) coordination center (<1 ps) and triplet–triplet energy transfer back to the BDP moiety (148 ps). These processes generated a triplet state localized at BDP, and the lifetime was 103.2 μs, much longer than the triplet-state lifetime of Pt-Ph (3.5 μs), a complex without the BDP moiety. Finally, Pt-BDP was used as a triplet photosensitizer for triplet–triplet annihilation (TTA) upconversion through selective excitation of the BDP unit or the Pt(II) coordination center at lower excitation energy. An upconversion quantum yield of up to 10% was observed with selective excitation of the BDP moiety, and a large anti-Stokes shift of 0.65 eV was observed upon excitation of the lower-energy band of the Pt(II) coordination center. We propose that using triplet photosensitizers with the ping-pong energy-transfer process may become a useful method for increasing the anti-Stokes shift of TTA upconversion.
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APPLIED SURFACE SCIENCE
·
2018
·
IF 4.439
Xinli Yang,Qiaojuan Jia,Fenghe Duan,Bin Hu,Minghua Wang,Linghao He,Yingpan Song,Zhihong Zhang
We synthesized a novel composite of multiwall carbon nanotubes (MWCNTs) decorated with MoS 2 quantum dots (MoS 2 QDs) and Ti 3 C 2 T x QDs (denoted by MoS 2 QDs@Ti 3 C 2 T x QDs@MWCNTs), of which MoS 2 QDs and Ti 3 C 2 T x QDs were separately prepared by exfoliating MoS 2 and Ti 3 C 2 T x MXene nanosheets by the hydrothermal method. It showed that the as–prepared MoS 2 QDs@Ti 3 C 2 T x QDs@MMWCNTs composite was rich in functional groups and exhibited homogeneous nanotube nanostructure by coupling with good electrochemical activity. Of note, the MoS 2 QDs@Ti 3 C 2 T x QDs@MWCNTs composite exhibited outstanding bifunctional electrocatalytic performances for oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR) in alkaline solution by combining the superior electrocatalytic activity of MoS 2 QDs and Ti 3 C 2 T x QDs and the excellent electrochemical performance of MWCNTs. The MoS 2 QDs@Ti 3 C 2 T x QDs@MMWCNTs catalyst exhibited a superior ORR activity to other non-Pt catalysts, giving a low Tafel slope (90 mV dec −1 ) and high half potential ( E 1/2 , 0.75 V), which was close to those of the commercial Pt/C (20%) catalyst (Tafel slope of 89 mV dec −1 , E 1/2 of 0.80 V). Additionally, the MoS 2 QDs@Ti 3 C 2 T x QDs@MMWCNTs also possessed good electro–oxidation performance for methanol in alkaline solution, giving a maximum methanol oxidation current density at 2.2 V of 160 A·g −1 . The results indicated that the combination of MoS 2 and Ti 3 C 2 T x QDs with MWCNTs can supply a potential for fabricating the bifunctional electrocatalysts for ORR and MOR.
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JOURNAL OF CATALYSIS
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2015
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IF 6.921
Xiaomei Ning,Hao Yu,Feng Peng,Hongjuan Wang
Effects of specific nitrogen functionality and oxidative functionalization of the surfaces of nitrogen-doped carbon nanotubes (NCNTs) on the interaction between Pt nanoparticles (NPs) and NCNTs have been systematically investigated. Their catalytic consequences were studied using aerobic oxidation of glycerol and electro-oxidation of CO as probing reactions. By transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), Raman spectroscopy, and X-ray diffraction (XRD), it was revealed that nitrogen dopant obviously enhanced the dispersion of Pt NPs. Strong interaction between Pt and NCNTs was observed. Graphitic nitrogen preferentially interacted with Pt NPs, evidenced by strong electron transfer from graphitic nitrogen as electron donor to metallic Pt NPs. The oxygen-containing groups introduced by H 2 O 2 oxidation of NCNTs may reduce the donor–acceptor interaction due to the electronegativity of oxygen. By changing the nitrogen amount of NCNTs and introducing oxygen groups, the electron enrichment of Pt NPs can be tuned. Superior catalytic activity was achieved over Pt/NCNTs in the oxidation of glycerol and electro-oxidation of CO, compared with conventional carbon nanotubes as support. Moreover, for both aerobic oxidation of glycerol and electro-oxidation of CO, it was observed that the intrinsic activity depended strongly on the electron enrichment of Pt NPs, ascribed to Pt4 f 7/2 (0) binding energy from XPS, suggesting a promising approach to improving catalytic activity by maximizing the interaction between Pt NPs and graphitic nitrogen sites.
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BIOSENSORS & BIOELECTRONICS
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2016
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IF 7.476
Ying Zhang,Wang Ren,Hong Qun Luo,Nian Bing Li
A new magnetic bead-based cascade amplification strategy for highly sensitive visual detection of proteins (thrombin as a model analyte) was developed by coupling target-triggered hybridization chain reaction (HCR) with the synergistic catalysis of DNA concatemer-mediated hemin/G-quadruplex DNAzymes and Pt nanozymes. Initially, the biotinylated primer DNA (P-DNA) was complementary with aptamer to form dsDNA which was further linked to streptavidin-coated magnetic bead (MB), thereby fabricating the expected MB-based aptasensor . In the presence of target TB, the aptamer was taken away from the aptasensor, and the free P-DNA immediately triggered HCR to spontaneously form DNA concatemer-directed nanochains with numerous DNAzymes and Pt nanoclusters (PtNCs) to achieve cascades signal amplification . The dual peroxidase mimetics catalyzed the H 2 O 2 -mediated oxidation of colorless 3,3′,5,5′-tetramethylbenzidine (TMB) into the colored TMB oxides (oxTMB), causing intensified color change of the chromogenic solution for the highly sensitive naked-eye detection of as low as 100.0 pM TB. In this strategy, the employment of magnetic separation and exonuclease III (Exo III)-assisted digestion of residual dsDNA minimized the background noise and avoided the false positive results, greatly improving the detection accuracy and sensitivity with a low limit of detection (LOD=15.0 pM). The proposed visual platform has promise for detecting various types of proteins with careful DNA sequence designs.
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Journal of Materials Chemistry C
·
2017
·Vol. 5
·期 9
·2466-2473
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IF 5.256
Shaochen Zhou,Mei Zhang,Fangyuan Yang,Fu Wang,Chuanyi Wang
A facile and green synthetic route is developed to prepare water soluble, green-fluorescent Pt, Au, Ag and Cu quantum clusters (QCs), employing innoxious L-histidine as a capping agent. These metal QCs give out emissions at 455–495 nm, with maximum excitation wavelengths ranging between 350 and 401 nm. Interestingly, these histidine-stabilized metal quantum clusters also possess non-linear optical properties like two-photon luminescence, which is detected when they are exposed to a femtosecond laser at 812 nm. Luminescence quantum yields of Pt (2.93%), Au (13.10%), Ag (6.97%) and Cu (8.29%) clusters are found to be distinctly different, and lifetime measurement results suggest that the emissions of metal clusters (4.59–7.39 ns) stem from singlet transitions among different electron energy levels rather than metal–ligand electron transfer behaviors. The Pt, Au, Ag and Cu quantum clusters have average sizes of 1.3–1.9 nm, and are mainly composed of 11, 9, 4 and 7 metal atoms, respectively, according to the electrospray ionization mass spectrometry results. Moreover, the as-prepared metal clusters are sensitive to aqueous ferric ions, both as highly selective fluorescent and colorimetric probes in a low and wide concentration range, and are promising in many biological applications.
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Cell Death & Disease
·
2017
·Vol. 8
·期 10
·e3095
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IF 5.965
Xu Junjie,Zheng Longbo,Chen Jiang,Sun Yin,Lin Hui,Jin Ren-an,Tang Minyue,Liang Xiao,Cai Xiujun
Although sorafenib is currently used as a standard treatment for advanced hepatocellular carcinoma, low response rate, transient and limited efficacy, primary and acquired resistance and negative side-effects gain increasing attentions, suggesting the need for better efficacious combination therapy. Here, we demonstrated that the sorafenib-induced or hypoxia-induced hypoxia inducible factor (HIF)-2 α could bind to an hypoxia responsive element within 500 bp region of androgen receptor (AR) promoter and thus transcriptionally suppress AR. Importantly, In vitro and In vivo studies suggested a specific and potent HIF-2 α inhibitor, PT-2385, could significantly enhance sorafenib efficacy by suppressing HIF-2 α , increasing AR and suppressing downstream pSTAT3/pAKT/pERK pathways. Clinical samples further confirmed the role of HIF-2 α and AR. It is promising that PT-2385 could alleviate the undesirable side-effects of sorafenib treatment by sorafenib-PT-2385 combination therapy, which may shed light for late-stage HCC patients.
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ELECTROCHIMICA ACTA
·
2017
·
IF 4.798
Bo Tang,Yuhui Lin,Zipeng Xing,Yaqiang Duan,Siyu Pan,Ying Dai,Jia Yu,Jinlong Zou
The problems of poor electrocatalytic activity and CO tolerance and high Pt-loading of the Pt-based catalysts are still needed to be solved for direct methanol fuel cells. In this study, porous MoS 2 /nitrogen-doped carbon (MoS 2 /CN X ) as Pt supports/co-catalyst for methanol oxidation reaction (MOR) is successfully prepared by using waste bagasse as carbon source. Various material characterization techniques and electrochemical tests are performed to investigate the relationship between structural characteristics and MOR activity. The highly porous structure of CN X can provide abundant binding sites for growing well-dispersed MoS 2 with coral-reef structure, which should facilitate the exposure of MoS 2 edge to improve co-catalytic activity of MoS 2 /CN X . Pt/MoS 2 /CN X displays a higher mass activity (1030.2 mA mg pt −1 ) than those of Pt/MoS 2 /C (710.1 mA mg pt −1 ) and commercial Pt/C (405.4 mA mg pt −1 ), owing to that MoS 2 /CN X can afford abundant attachment sites to anchor Pt to enlarge the available electrochemically active area (111.2 m 2 g −1 pt ) for MOR. With the introduction of porous CN X , more active sites on MoS 2 edges are exposed out to dissociate water molecule for eliminating adsorbed CO-species on the active sites of Pt, which is conductive to enhance the durability and CO tolerance of Pt/MoS 2 /CN X . Furthermore, MoS 2 /CN X with high specific surface area (451.38 m 2 g −1 ) can offer sufficient oxygen-containing functional groups to facilitate the oxidation of intermediates (CO-species) on the active Pt sites, which can also promote the accessibility of methanol to the electroactive surface. These results provide a promising strategy for the design of highly active Pt support/co-catalyst to minimize Pt usage.
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Advanced Materials Interfaces
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2017
·Vol. 4
·期 12
·1700005
·
IF 4.279
Juan Wang,Jia Wei Chen,Jia Dong Chen,Han Zhu,Ming Zhang,Ming Liang Du
Well-dispersed Pt Cu alloy nanoparticles (NPs) with a diameter of only ≈2 nm encapsulated in carbon nanofibers (CNFs) are synthesized using electrospinning technology followed by a graphitization process in a chemical vapor deposition furnace. Distinctly, even with a small amount of Pt, the Pt Cu/CNFs-1:2 catalyst possesses outstanding hydrogen evolution reaction (HER) activity, including small overpotential, long-term stability, and a high exchange current density as well as large double layer capacitance ( C dl ). The excellent HER performance of the Pt Cu/CNFs-1:2 catalyst is attributed to the synergistic interaction between Pt and Cu, the uniform distribution of the alloy NPs and the use of CNFs with 3D architectures. This development may provide a simple, efficient, and green synthesis method to design bi- or multimetal alloys for use as the cathode electrocatalysts for the HER or other electrocatalytic devices.
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ANALYTICA CHIMICA ACTA
·
2021
·
IF 6.558
Zhenxing Wang,Hongli Zhao,Kaicha Chen,Hongyuan Li,Minbo Lan
Signal amplification is crucial to improve the sensitivity for the electrochemical detection of cardiac troponin I (cTnI), one of the ideal biomarkers for early acute myocardial infarction (AMI) diagnosis. Herein, we developed a novel signal amplification strategy to construct a sandwich-type electrochemical aptasensor for the detection of cTnI. Core-shell [email protected] dendritic bimetallic nanoparticles loaded on melamine modified hollow mesoporous carbon spheres ( [email protected] DNs/NH 2 -HMCS) was prepared as labels to conjugate with thiol-modification DNA aptamers probe for signal amplification. While introducing numerous amino groups, the melamine functionalized hollow mesoporous carbon spheres (NH 2 -HMCS) retained the edge-plane-like defective sites for the adhesion and electrocatalytic reduction of H 2 O 2 . With the unique characteristics of NH 2 -HMCS, it not only enhanced the dispersity and loading capacity of core-shell [email protected] dendritic bimetallic nanoparticles ( [email protected] DNs), but also improved the stability of bonding by the affinity interaction between [email protected] DNs and amino groups of melamine. Meanwhile, the synergistic catalysis effect between [email protected] DNs and NH 2 -HMCS significantly enhanced the electrocatalytic reduction of H 2 O 2 and further amplified the signal. Under optimal conditions, this recommended aptasensor for cTnI detection displayed a wide dynamic range from 0.1 pg/mL to 100.0 ng/mL and a low detection limit of 15.4 fg/mL (S/N = 3). The sensor also successfully realized the analysis of cTnI-spiked human serum samples, meaning potential applications in AMI diagnosis.
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TALANTA
·
2021
·
IF 6.057
Jie Zheng,Min Zhu,Jiao Kong,Zimu Li,Jianming Jiang,Yachao Xi,Fang Li
Herein, a simple microfluidic paper-based analytical device (μPAD) by using platinum nanoparticles (Pt NPs) as highly active peroxidase mimic for simultaneous determination of glucose and uric acid was fabricated. The μPAD consisted of one sample transportation layer, four paper-based detection chips, and two layers of hydrophobic polyethylene terephthalate (PET) films. The four detection chips were immobilized with various chromogenic reagents, Pt NPs, and specific oxidase (glucose oxidase or uricase). H 2 O 2 generated by specific enzymatic reactions could oxidize co-immobilized chromogenic reagents to produce colored products by using Pt NPs as efficient catalyst. The multi-layered structure of μPAD could effectively improve the color uniformity and color intensity. Total color intensity from each two detection chips modified with distinct chromogenic reagents were used for quantitative analysis of glucose and uric acid, respectively, resulting in significantly improved sensitivity. The linear range for glucose and uric acid detection was 0.01–5.0 mM and 0.01–2.5 mM, respectively. Satisfied results were obtained for glucose and uric acid detection in real serum samples. An easy-to-use smartphone APP was developed for convenient and intelligent detection. The developed μPAD integrated with smartphone as detector holds great applicability for simple and portable on-site analysis.
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Analytical Methods
·
2018
·Vol. 11
·期 4
·443-453
·
IF 2.073
Pramod K. Kalambate,Yankai Li,Yue Shen,Yunhui Huang
In this work, a novel highly sensitive electrochemical sensing platform has been developed for simultaneous determination of anticancer drugs doxorubicin (DOX) and dasatinib (DAS) by means of mesoporous Pd@Pt core–shell nanoparticles supported on MWCNT (Pd@Pt/MWCNT). The electrochemical behaviour of the drugs was assessed through cyclic voltammetry, while simultaneous determination was carried out using adsorptive stripping square wave voltammetry (AdSSWV). Under optimized conditions, the method exhibits linear responses towards simultaneous determination of DOX and DAS in the concentration ranges of 4.4–8580 nM and 38–9880 nM, with detection limits of 0.86 and 6.72 nM, respectively. Furthermore, the proposed platform was successfully used for reliable determination of DOX and DAS in urine and blood serum samples with good accuracy and precision. The satisfactory recoveries obtained in blood serum and urine samples showed the potential for application of the proposed platform in quality control in the pharmaceutical industry, clinical analysis and optimization of chemotherapeutic treatment. We found that the established sensor has several advantages in terms of high sensitivity and selectivity, ease of preparation, short analysis time, long-term stability and fast response.
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